Polymer Degradation and Stability 59 (I 998) 263-212

(c) 1998 Published by Elsevier Science Limited. All rights reserved

Printed in Northern Ireland
PII: SO141-3910(97)00156-O 0141.3910/98/$19.00

Properties and applications of Mater-Bi

starch-based materials
Catia Bastioli”
Novamont S.p.A., Via G. Fauser, 8, I-28100 Novara, Italy

(Accepted 12 July 1997)

Novamont is generally recognized as a pioneer in the sector of starch-based bio-

degradable materials. It started its research activity in 1989, and now has four
classes of materials, A, Z, V, and Y, sold under the Mater-Bi trademark, con-
taining starch and differing in their synthetic components.
This paper revises the main results obtained by Novamont in the field of ther-
moplastics and complexed starch in the presence of specific synthetic polymers,
and aspects, such as processability, physico-chemical and physico-mechanical
properties, composting behavior and future market perspectives of Mater-Bi
products.
Moreover, the paper considers aspects such as in-use performances and bio-
degradation behavior of Mater-Bi bags for the separate collection of organic and
yard waste, the first real industrial product in the sector of biodegradable
materials introduced in the market by Novamont since 1992. 0 1998 Published
by Elsevier Science Limited. All rights reserved

1 INTRODUCTION economical. Technologies, such as cornposting

The management of solid waste disposal with
regard to the decreasing availability of landfills, the
litter problem and the pollution of the marine
environment is becoming very urgent in indus-
trialized countries and may extend very quickly to
developing countries.
A solution is the valorization of waste as a
resource through its separation into specific frac-
tions, to be transformed into new products with a
certain market value. Technological aspects, such
as the development of safer and more efficient
recycling technologies and the development of
materials which are easy to reuse or recycle and of
biodegradable materials, can significantly con-
tribute to the solution of the problem.
Biodegradable polymers constitute a loosely
defined family of polymers that are designed to be
degraded by living organisms. They offer a possi-
ble alternative to traditional non-biodegradable
polymers when recycling is impractical or not
*Fax: 39 321 699601; e-mail: novamont.bastioli@novara.
alpcom.it
263
used for the disposal of food and yard waste,
accouning for 2540% of the total municipal solid
waste, are the most suitable for the disposal of
biodegradable materials together with soiled or
food-contaminated paper.
International organizations, such as the Amer-
ican Society for Testing and Materials (ASTM), in
connection with the Institute for Standards
Research (ISR), the European Standardisation
Committee (CEN), the International Standardisa-
tion Organisation (ISO), the German Institute for
Standardisation (DIN), the Italian Standardization
Agency (UNI), the Organic Reclamation and
Cornposting Association (ORCA), are all actively
involved in developing * definitions and tests for
biodegradability in different environments and
compostability.‘,*
Although a standard world-wide definition for
biodegradable plastics has not been established,
nevertheless all the definitions already in place
(ASTM, CEN, ISO) correlate the degradability of
a material to a specific disposal environment and to
a specific standard test method which simulates
this environment in a time period which determines
its classification.
264 C. Rastioli
According to this approach CEN, ORCA, UN1
and DIN have defined, at draft level, the basic
requirements for a product to be declared
compostable based on:
l Complete biodegradability of the product,
measured through respirometric tests like
ASTM D5338-92, ISO/CD14855 and corre-
sponding CEN draft or the modified Sturm test
ASTM D5209, in a time period compatible with
the cornposting technology (a few months);
l Disintegration of the material during the
fermentation phase;
l No negative effects on compost quality and in
particular no toxic effects of the compost and
leachates on terrestrial and aquatic organisms;
l Control of laboratory-scale results on pilot/
full-scale cornposting plants.
These requirements set forth a common base for
a universal marking system to readily identify
products to be composted.
Starch-based materials are now industrial prod-
ucts and are leading the still small market of bio-
degradable products, whereas aliphatic polyesters,
another promising class of materials, are just at the
development stage.
The market potential for biodegradable products
in the next 5 years can be estimated at approxi-
mately 30 00@-40 000 ton/year in Europe. Amer-
ican and Japanese markets are of great potential,
but are still at a very early stage of development,
with the exception of starch-based loose-fillers.
This paper reviews the state of the art of thermo-
plastic starch and the results obtained by Novamont
on thermoplastic starch complexed with synthetic
hydrophylic/hydrophobic copolymers, on thermo-
plastic starch blended with non-compatible syn-
thetic polymers, and on thermoplastic starch
partially complexed with non-compatible or
slightly compatible synthetic polymers.
The four classes of Mater-Bi products currently
available on the market are also described in terms
of processability, physico-chemical and physico-
mechanical properties and biodegradation behavior.
2 NOVAMONT: GENERAL INFORMATION
Novamont is an innovation-oriented company,
able to develop and apply advanced technologies
to natural raw materials for the solution of envi-
ronmental problems. From the very beginning,
Novamont followed an approach based on three
main points:
l use abundant, inexpensive, natural raw mat-
erials, available annually from different crops,
in excess of current market needs in USA and
Europe, like starch, proteins, cellulose, vege-
table oils;
a take advantage of the skills of an experienced
interdisciplinary team of ‘Materials Science’;
l engineer tailor-made materials for specific
applications, identified by means of a close
contact between R&D and the market.
The present objective is the production of a new
generation of plastic-like materials from natural
sources, which retain their properties while in use and
completely biodegrade when properly discharged.
The Novamont approach gave effective results
mainly in the area of starch-based materials with
significant achievements on starch destructuriza-
tion, complexation and compatibilization, in the
presence of specific synthetic and natural polymers
and additives, and on the engineering of products
with a wide range of properties.
The behavior of starch-based materials has been
deeply studied in terms of processability, physico-
chemical and physico-mechanical properties and
biodegradation trend.
The production capacity of Novamont today is
8000 ton/year.
The technology used is very flexible and permits
adaptation of the plant capacity to the market
needs, with minor investments and in a short
period of time.
3 STARCH-BASED MATERIALS: STATE OF
THE ART
Starch is an inexpensive abundant product avail-
able annually from corn and other crops. It is
totally biodegradable in a wide variety of environ-
ments and can permit the development of totally
degradable products for specific market needs.
Degradation or incineration of starch products
recycles the atmospheric CO2 trapped by starch-
producing plants during their growth, thus closing
the biological carbon cycle.
Starch is constituted by two major components:
amylose, a mostly linear alpha-D-( l-4)-glucan and
amylopectin, an alpha-D-( l-4) glucan which has
alpha-D-(1-6) linkages at the branch point. The
 Properties and applications of Mater-Bi starch-based materials
linear amylose molecules of starch have a mole-
cular weight of 0.2-2 million, while the branched
amylopectin molecules have molecular weights as
high as 100-400 million.3T4
In nature, starch is found as crystalline beads of
approximately 15 -100 pm in diameter, in three
crystalline modifications designated A (cereal), B
(tuber), and C (smooth pea and various beans), all
characterized by almost perfect left-handed, six-
fold double helices.
3.1 Thermoplastic starch
Starch can be made thermoplastic according to a
technology very similar to extrusion cooking.
Extrusion cooking and forming is characterized by
sufficient work and heat being applied to a cereal-
based product to cook or gelatinize completely ail
the ingredients. Equipment used for high pressure
extrusion heats materials during processing, and
continually compresses them.
Thermoplastic starch products with different
viscosity, water solubility and water absorption
have been prepared by altering the moisture con-
tent of the raw product and the temperature or the
pressure in the extruder. A thermoplastic starch
can be solubilized without any formation of mal-
todextrins, and the extent of solubilization depends
on the extrusion temperature, the moisture content
of the starch before extrusion and the amylose/
amylopectin ratio.5-9
Thermoplastic starch alone can be processed as a
traditional plastic; its sensitivity to humidity, how-
ever, makes it unsuitable for most applications.
The main use of thermoplastic starch alone is in
soluble compostable foams, such as loose-fillers,
expanded trays, shape molded parts, expanded
layers, as a replacement for polystyrene.
4 THERMOPLASTIC STARCH COMPOSITES
Starch can be destructurized in combination with
different synthetic polymers to satisfy a broad
spectrum of market needs.1@26 Thermoplastic
starch composites can reach starch contents higher
than 50%.
Novamont discovered that thermoplastic starch
in combination with synthetic polymers can gen-
erate three different families of materials.
1. Thermoplastic starch complexed with syn-
thetic copolymers containing hydrophylic and
265
hydrophobic units (i.e. copolymers of vinyl-
alcohol, polyester-urethanes, ethylene-acrylic
acid copolymers, etc.).
2. Thermoplastic starch blended with incompat-
ible synthetic polymers (cellulose derivatives,
aliphatic polyesters, etc.)
3. Partially complexed and/or compatibilized
thermoplastic starch blended with incompat-
ible or slightly compatible synthetic polymers.
The biodegradation behavior of the different
products is mainly influenced by the biodegrad-
ability of the synthetic component, although the
presence of starch can significantly influence the
biodegradation rate of intrinsically biodegradable
synthetic components.
5 THERMOPLASTIC STARCH COMPLEXED
WITH SYNTHETIC COPOLYMERS
As an example, starch/vinyl alcohol copolymer
systems, 27 depending on the processing conditions,
on starch type and on copolymer composition, can
generate a wide variety of morphologies and prop-
erties as a result of the extent of a complex formed
between amylose and the synthetic molecules
(Figs 1 and 2). Second derivative IR studies suggest
for the amylose configuration a six-folded single
helix identified as a ‘V’ structure.
A model has been proposed considering large
individual amylopectin molecules interconnected at
several points per molecule as a result of hydrogen
bonds and entanglements by chains of amylose/
vinyl alcohol copolymer V complexes.
Fig. 1. Droplet-like
structure of thermoplastic corn starch/
EVOH system (5050 w/w on a dry basis), after disgregation in
boiling water.
266
Fig. 2. Layered structure of thermoplastic waxy maize/EVOH
system (50:50 w/w on dry basis) after 3 days of soil burial.
This structure has been defined in the literature
as ‘interpenetrated’ and makes starch completely
insoluble.27
The biodegradation rate of starch in these mat-
erials is inversely proportional to the content of
amylose/vinyl alcohol copolymer complex (Fig. 3).
The products based on starch/polyethylene-vinyl
alcohol (EVOH) show mechanical properties good
enough to meet the needs of specific industrial appli-
cations. Their moldability in tim blowing, injection
molding, blow molding, thermoforming, foaming,
etc. is comparable with that of traditional plastics
such as PS, ABS, LDPE.28 The main limitations of
these materials are in their high sensitivity to low
humidities, with consequent enbrittlement.
Fig. 3. Weight loss of thermoplastic corn starch/EVOH (60:40) films in a soil burial test as a function of time and of amylose
content: (a) 70% amylose; (b) 25% amylose; (c) 5% amylose.
C. Bastioli
The biodegradability of these composites has
been demonstrated in different environments.29
The degradation rate of 2-3 years in a watery
environment remains too slow for considering
these materials compostable (Fig. 4).
6 THERMOPLASTIC STARCH NOT
COMPLEXED OR PARTIALLY COMPLEXED
WITH INCOMPATIBLE POLYMERS
Starch can also be destructurized in the presence of
more hydrophobic polymers such as aliphatic
polyesters.30
It has been found that the blending of starch
with aliphatic polyesters improves their processa-
bility and biodegradation behavior. Particularly
suitable polyesters are poly-c-caprolactone and its
copolymers, or polymers at higher melting point
formed by the reaction of glycols as 1,4 butandiol
with succinic acid or with sebacic acid, adipic acid,
azelaic acid, decanoic acid or brassilic acid. The
presence of compatibilizers between starch and ali-
phatic polyesters, such as amylose complexed with
aliphatic polyesters or with polymers partially or
completely compatible with polyesters,31 starch
grafted polyesters, chain extenders like diisocya-
nates, epoxides, etc., can improve the properties of
starch composites.
These types of materials are characterized by
excellent compostability, good mechanical proper-
ties and reduced sensitivity to water.
Time (days)
 Properties and applications of Mater-Bi starch-based materials
Fig. 4. Weight loss (wl) of Mater-Bi AIOSH (A class) (thermoplastic
(SCAS) test conditions as a function of time (t).
Fig. 5. Microstructure of a thermoplastic starch blended with
poly-•-caprolactone. The starch component has been removed
by etching with 1N HCl.
Thermoplastic starch can also be blended with
cellulose derivatives, as reported in the literature.29
Thermoplastic starch in this case can be found as a
dispersed form (Fig. 5).
7 PLASTICIZED THERMOPLASTIC
STARCH
The combination of gelatinized starch with a solu-
ble polymer, such as poly(viny1 alcohol) (PVOH)
and/or poly(alkylene glycols), has been widely
considered since 1970. In recent years, thermo-
plastic starch/PVOH has been mainly studied for
producing starch-based loose-fillers as a replace-
ment for expanded polystyrene.32-35
267
starch/EVOH 60:40) under semicontinuous activated sludge
The results obtained in the field of thermoplastic
starch in combination with polymers or copoly-
mers of vinyl alcohol and with aliphatic polyesters
and copolyesters in terms of biodegradation kinet-
ics, mechanical properties and reduced sensitivity
to humidity make these materials ready for a real
industrial development starting from film, foam
and injection molding applications. The present
global market is about 12 000 tons/year.
Main producers are Novamont with the Mater-
Bi trademark, ENPAC and National Starch.
8 MATER-B1 PRODUCTS
Under the Mater-Bi [67-69] trademark, Novamont
today produces four classes of biodegradable
materials (Table l), all based on starch and differ-
ing in synthetic components.
1 Class Z :Biodegradable and compostable,
mainly for films and sheets. The biodegrada-
tion behavior is reported in Figs 6 and 7. They
contain thermoplastic starch and poly+
caprolactone and were introduced into the
market at the beginning of 1992. The micro-
structure of the products belonging to this
class can be very different, ranging from ther-
moplastic starch dispersed in the synthetic
component (Fig. 5) as in the case of Mater-Bi
ZIOIU, to thermoplastic starch in a semi-
continuous phase, as in the case of Mater-Bi
ZF03U/A.
2. Class V: Biodegradable, compostable and
soluble, as a replacement for polystyrene
268 C. Bastioli

Table 1. Mater-Bi: classes and grades

Z class l Biodegradable and compostable mainly for films and sheets.

l Biodegradation time of 2@-45 days in composting conditions.
l Made of thermoplastic starch and poly-t-caprolactone.
Grade Technology use
ZF03U/A Film blowing Bags, nets, paper lamination, mulch films, twines,
wrapping film...
ZF02U/A Film blowing Diaper backsheets, paper lamination...
ZIOl u Film blowing/extrusion/casting injection General purposes, wrapping film...
molding
ZIO 1U/T Extrusion/calandering/injection molding Thermoformed and injected items...

Y class l Biodegradable and compostable for rigid and dimensionally stable injection molded items.
. Biodegradation time of about 4 months in composting conditions and 30 days in anaerobic
conditions (1 mm in thickness).
l Made of thermoplastic starch and cellulose derivative.

Grade Technology Use

YIOlU Injection molding Cutlery, boxes, flowers pots, seedling plantertrays,
golf tees, vending cups, pens...

V class l Biodegradable, compostable and soluble for rigid and espanded items.
l Biodegradation time even shorter than Z grades.
l Content of thermoplastic starch more than 85%.

Grade Technology Use

PE02U Foaming Loose fillers and packaging foams as a replacement
of polystyrene...
PE03U Injection molding SoIuble cotton swabs, soluble items...

A class l Biodegradable, not compostable, mainly for molded items.

l Biodegradation time of about 2 years in an environment simulating a sewage sludge treatment plant.
l Made of starch and ethylene vinyl-alcohol copolymer, used in applications where compostability is
not required.

‘3100
8 90
e 80
0" 70
ti 60
.g 50
7 40
; 30 -m-ZFO3UIA

z 20
E 10
2
0 0
0 10 20 30 40 50 60
Time (Days)
_____~

Fig. 6. Aerobic biodegradation of Mater-Bi products of class Z under controlled composting conditions (ASTM D 5338-92), in
comparison with pure cellulose (test performed by VTT Institute, Finland).

packaging foams. Their biodegradation beha-
vior in a watery environment is reported in
Fig. 7. They have a starch content > 85% and
can be defined as thermoplastic plasticized
starch.
3. Class Y: Biodegradable and compostable,
for rigid and dimensionally stable injection
molded items; they contain raw materials all
from natural origin, such as thermoplastic
starch in a dispersed form and cellulose deriva-
tives. Their biodegradation behavior in different
environments is reported in Figs 7-9. Their
mechanical properties (Table 2) and mold-
ability are very close to those of polystyrene.
 Properties and applications of Mater-Bi starch-based materials 269

20 30 ‘lo 50
Time ( Days)

Fig. 7. Aerobic biodegradation of different Mater-Bi grades in the presence of municipal sewage sludge (ASTM D 5209-91 test).

100
90
g 80
- 70
oe
s 6o
E 50
I 40
E 30
20
10
0
0 20

Time (days)

Fig. 8. High solid anaerobic digestion of Mater-Bi YIOI U in comparison with cellulose powder (ASTM D5511-94 performed by
OWS, Belgium).

100 , oc

2 80
: 56
; 60

g 40

s 20

0 --t
30 60 90
Time (Davsb

Fig. 9. Weight loss of Mater-Bi YIOlU under cornposting conditions (test method described in Ref. 36).

4. Class A: Biodegradable, non-compostable main uses are in sectors where compostability

materials (biodegradation time of 2 years in a is not required.
liquid environment (Fig. 4). They contain Novamont has recently launched two new grades
thermoplastic starch heavily complexed with of Mater-Bi for films belonging to class Z, ZIOlU
ethylene-vinyl alcohol copolymers. Their and ZF03U/A, which have the ‘OK COMPOST’
270 C.Bastioli

Table 2. Some physical properties of Mater-Bi YIOlU in comparison with traditional plastics
Test Procedure Unit YIOlU PS
Density Pycnometer g/cm3 1.35 1.04t 1.09
Melt flow rate ASTM D1238 g/lOmin 10+15 8e-12
(at 19O”C, load 5 kg)
Tensile strength ASTM D882 Mpa 25t30 35+64
Elongation at brake ASTM D882 % 2~6 le2.5
Tensile modulus ASTM D882 Mpa 2100+2500 2800+3500

Table 3. Some physical properties of Mater-Bi grades belonging to Z class, in comparison with traditional plastics
Test Procedure Unit ZF03U/A ZIOIU LDPE

MFI ASTM D1238 g/lOmin 4-5.5 1.5 0.1-22

Strength at break ASTM D882 MPa 31 28 8-10
Elongation at break ASTM D882 % 886 780 15&600
Young modulus ASTM D882 MPa 185 180 1O&200
Tear strength ASTM D1938
Primer N/mm 68 55 60
Propagation N/mm 68 55 60

certificate released by AIB-Vincotte Inter, an
international company of auditing.
The assignment criteria of the ‘OK COMPOST’
label follow the ORCA Compostability Criteria
and the draft guidelines currently under discussion
by international and national committees, such as
CEN, ISR/ASTM, ISO, DIN, UNI.
Moreover, the biodegradability of the two mat-
erials in cornposting conditions has been measured
by VTT, Finland (Fig. 6) and by other institutes.
Data of biodegradability in different environments
are reported in Figs 6, 7 and 10. Their mechanical
properties are very similar to those of low density
polyethylene (Table 3).
Fig. 10. Weight loss of Mater-Bi ZIOIU (class Z) under com-
posting conditions.
These Mater-Bi materials are industrial products
designed for films and layers. An important exam-
ple of a successful application of these two grades
is represented by the compostable bags for organic
and yard waste collection. The films and bags can
be produced by means of traditional film blowing and
sealing equipment for low density polyethylene with
minor modifications, reaching similar productivities.
Bags of different sizes are already used by millions of
European citizens for the separate collection of the
organic fraction of MSW to be composted.
Novamont’s entrance into this market sector has
been preceded by a comprehensive study on the
behaviour of Mater-Bi bags in different compost-
ing plants (from static windrows to rotary fer-
menting reactors) and in ‘in-use’ conditions, in co-
operation with some European municipalities like
Furstenfeldbruck (Germany), Korneuburg (Aus-
tria), Trento and Bellusco (Italy). The preliminary
study has been completed in about 2 years, from
1992 to 1994. A summary of this preliminary
activity was presented at the International Con-
ference ‘The Science of Cornposting’ in 1995.37
Both the in-use performance and compostability
of Mater-Bi bags in full-scale cornposting facilities
have been fully satisfactory.
Besides cornposting and yard waste bags, other
main uses of Mater-Bi products are in the field of
short-life applications, such as shopping bags
(Fig. 1l), mulch film, film for wrapping, loose-fillers
(Fig. 12) and expanded shape molded parts as a
replacement for polystyrene, soluble cotton swabs,
nursery pots, cutlery, etc.
 Properties and applications of Mater-Bi starch-based materials
Fig. 11. Composting bag made of Mater-Bi of class Z.
Fig. 12. Loose fillers made of Mater-Bi of class V.
9 CONCLUSIONS
Mater-Bi products made of thermoplastic starch in
combination with polymers of vinyl alcohol, with
aliphatic polyesters and copolyesters and with cel-
lulose and starch derivatives are already available
at an industrial level. Their biodegradation rate is
similar to that of cellulose and their mechanical
properties close to those of traditional plastics like
polyethylene and polystyrene. Their reduced sensi-
tivity to humidity makes these materials particu-
larly suitable for the production of films, injection
molded items and foams.
271
Mater-Bi products are the result of a significant
investment made by Novamont in research and
development, testified to by the wide patent port-
folio and by the leading position in the small mar-
ket of biodegradable materials. In spite of these
positive results, thermoplastic starch-based materi-
als are still at an early stage of development with
many opportunities still to be taken.
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